JP7061622B2 - Methods and systems for removing harmful compounds from flue gas using fabric filter bags with SCR catalysts - Google Patents
Methods and systems for removing harmful compounds from flue gas using fabric filter bags with SCR catalysts Download PDFInfo
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Description
本発明は、オフガスおよび煙道ガス(燃料排ガス)から排出される粒子状物質および窒素酸化物(NOx)を還元するための方法およびシステムに関する。特に、本発明の方法およびシステムは、低いガス温度でNOxの還元の改善をもたらす。 The present invention relates to methods and systems for reducing particulate matter and nitrogen oxides (NOx) emitted from off-gas and flue gas (fuel exhaust). In particular, the methods and systems of the invention provide improved NOx reduction at low gas temperatures.
様々な燃焼設備、例えば、固体または液体火力発電所(solid or liquid fired power plants)のボイラー、ガス石油火力発電機またはセメントキルン、バイオ燃料燃焼プラント、およびごみ焼却場からの煙道ガスは、多数の環境上問題のある、またはさらには毒性のある化合物を含有する。これらは、粒子状物質およびNOxを含む。 A large number of boilers, gas oil-fired generators or cement kilns, biofuel combustion plants, and flue gas from various combustion facilities, such as solid or liquid field power plants. Contains environmentally problematic or even toxic compounds. These include particulate matter and NOx.
粒子フィルターおよび煙道ガスの触媒浄化の使用は、粒子状物質およびNOxの量を低減するので、一般に環境に有益である。ほとんどの地域において、煙道ガス中のNOxの還元が法規で必要とされている。 The use of particle filters and catalytic purification of flue gas is generally beneficial to the environment as it reduces the amount of particulate matter and NOx. In most areas, the reduction of NOx in flue gas is required by law.
ファブリックフィルターバッグは、多くの業界において、煙道ガスおよびプロセスガスからの粒子状物質の除去に広く用いられている。これらは、最も効率的な種類の集塵機である。 Fabric filter bags are widely used in many industries for the removal of particulate matter from flue gases and process gases. These are the most efficient types of dust collectors.
上記のように、オフガスおよび煙道ガスは、複数の汚染物質、とりわけ窒素酸化物を各国の法規に応じて除去または低下されるべき濃度で含有する場合が非常に多い。いくつかの従来の方法がこの目的のために利用できる。いかなる場合でも、ファブリックフィルターバッグの上流/下流に追加のユニットを設置し、操作する必要がある。 As mentioned above, off-gas and flue gases very often contain multiple pollutants, especially nitrogen oxides, in concentrations that should be removed or reduced according to national legislation. Several conventional methods are available for this purpose. In any case, additional units need to be installed and operated upstream / downstream of the fabric filter bag.
参照によりその全体が本明細書に含まれる、同時継続中の米国仮特許出願第2017/0080387号(特許文献1)の譲渡人により、SCR活性触媒で触媒されたフィルターバッグが開示されている。オフガスまたは煙道ガスがこれらのフィルターバッグを通ると、フィルターバッグにより、濃縮NOxおよび粒子状物質が還元または除去される。 The assignor of US Provisional Patent Application No. 2017/0080387 (Patent Document 1), which is incorporated herein by reference in its entirety, discloses a filter bag catalyzed by an SCR active catalyst. When off-gas or flue gas passes through these filter bags, the filter bags reduce or remove concentrated NOx and particulate matter.
フィルターバッグを構成する繊維の組成により、これらは、250℃未満の温度で操作されねばならない。 Due to the composition of the fibers that make up the filter bag, they must be operated at temperatures below 250 ° C.
NOxの選択的触媒還元(SCR)において、酸化窒素化合物は、触媒上でアンモニアなどの還元剤と反応することにより無害な窒素と水に選択的に還元される。 In the selective catalytic reduction (SCR) of NOx, the nitrogen oxide compound is selectively reduced to harmless nitrogen and water by reacting with a reducing agent such as ammonia on the catalyst.
フィルターバッグの組成により必要とされる低いガス温度は、SCRによるNOxの除去において問題に直面する。 The low gas temperature required by the composition of the filter bag faces problems in the removal of NOx by SCR.
公知のSCR触媒の問題は、250℃未満のガス温度で効率が相対的に低いことである。 The problem with known SCR catalysts is their relatively low efficiency at gas temperatures below 250 ° C.
本発明は、煙道ガスダクトの外側でNO2を生成し、調製されたNO2をいわゆる「Fast」SCR反応(fast SCR reaction)を促進する量で煙道ガスに注入することに基づく。第1のステップでの貴金属含有触媒上でのNH3のNOへの酸化、その後、第2のステップでのNOのNO2への酸化により、NO2をNH3から生成できる。 The present invention is based on producing NO 2 outside the flue gas duct and injecting the prepared NO 2 into the flue gas in an amount that promotes the so-called "Fast" SCR reaction. NO 2 can be produced from NH 3 by the oxidation of NH 3 to NO on the noble metal-containing catalyst in the first step and then to NO 2 of NO in the second step.
「Fast」SCR反応:2NH3+NO+NO2→2N2+3H2Oにより、煙道ガス中等モル量のNOとNO2で、SCR反応は著しく促進され得、低温活性は著しく上昇し得ることが公知である。 It is known that "Fast" SCR reaction: 2NH 3 + NO + NO 2 → 2N 2 + 3H 2 O can significantly promote the SCR reaction and significantly increase the low temperature activity with a medium molar amount of NO and NO 2 in the flue gas. be.
したがって、第1の態様において、本発明は、燃焼設備の煙道ガスから窒素酸化物を除去する方法であって、
煙道ガスに添加されたアンモニアそれ自体またはその前駆体の形態のいずれかの存在下で、煙道ガスを窒素酸化物の選択的還元用触媒で触媒された1つもしくは複数のファブリックフィルターバッグに通すステップ;
1つもしくは複数のファブリックフィルターバッグの上流で、二酸化窒素を含有する排ガスを煙道ガスに注入するステップ;
酸化触媒の存在下で、アンモニアまたはその前駆体を酸素含有雰囲気下で触媒酸化して、一酸化窒素および酸素を含有する排ガスにするステップ、
排ガスを周囲温度まで冷却し、冷却された排ガス中の一酸化窒素を酸化して、二酸化窒素を含有する排ガスにするステップ
により、二酸化窒素を含有する排ガスを得るステップ
を含む、方法を提供する。
Therefore, in the first aspect, the present invention is a method for removing nitrogen oxides from the flue gas of a combustion facility.
In the presence of either ammonia itself added to the flue gas or in the form of its precursor, the flue gas is catalyzed by a catalyst for the selective reduction of nitrogen oxides into one or more fabric filter bags. Steps to pass;
Injecting nitrogen dioxide-containing exhaust gas into flue gas upstream of one or more fabric filter bags;
A step of catalytically oxidizing ammonia or its precursor in the presence of an oxidation catalyst in an oxygen-containing atmosphere to produce an exhaust gas containing nitric oxide and oxygen.
Provided is a method comprising a step of obtaining a nitrogen dioxide-containing exhaust gas by cooling the exhaust gas to an ambient temperature and oxidizing the nitric oxide in the cooled exhaust gas to the nitrogen dioxide-containing exhaust gas.
公知の方法およびシステムの問題は、本明細書で上述したように250℃未満の煙道ガス温度でSCR触媒の効率が相対的に低いことである。この問題は、「Fast」SCR反応を促進するために低温でNO2を煙道ガスに注入することを伴う本発明により解決される。この反応は、低温でのSCRの促進に関与する。 A problem with known methods and systems is the relatively low efficiency of SCR catalysts at flue gas temperatures below 250 ° C. as described herein. This problem is solved by the present invention involving injecting NO 2 into the flue gas at low temperatures to facilitate the "Fast" SCR reaction. This reaction is involved in promoting SCR at low temperatures.
煙道ガス温度が250℃超のとき、SCR触媒は十分な効率を有し、ガス温度が250℃に到達すると、NO2の煙道ガスへの注入は中断され得る。 When the flue gas temperature is above 250 ° C, the SCR catalyst has sufficient efficiency, and when the gas temperature reaches 250 ° C, the injection of NO 2 into the flue gas can be interrupted.
煙道ガスダクトの外側でのアンモニアのNOへの酸化は、通常、酸素含有雰囲気の存在下で、250~800℃の反応温度で、微量成分として典型的には白金または白金と他の貴金属との合金などの貴金属触媒を有する反応器中で行われる。 Oxidation of ammonia to NO outside the flue gas duct is usually in the presence of an oxygen-containing atmosphere at a reaction temperature of 250-800 ° C., typically platinum or platinum as a trace component with other noble metals. It is carried out in a reactor having a noble metal catalyst such as an alloy.
必要とされる反応温度にするために、酸化反応器は、例えば、通電加熱または誘導加熱により加熱され得る。 To reach the required reaction temperature, the oxidation reactor can be heated, for example, by energization heating or induction heating.
一実施形態において、酸素含有雰囲気は高温再循環ガス(hot recirculated gas)を含み、これはひいてはさらに、酸化反応器の加熱負荷の一部を担う。 In one embodiment, the oxygen-containing atmosphere comprises a hot recirculated gas, which in turn is part of the heating load of the oxidation reactor.
平衡反応 Equilibrium reaction
本明細書で使用する用語「周囲温度」は、本発明の方法およびシステムを使用する燃焼設備の周辺で優勢な任意の温度を意味するものとする。典型的には周囲温度は-20℃~40℃である。 As used herein, the term "ambient temperature" is used to mean any temperature predominant around a combustion facility that uses the methods and systems of the invention. Typically, the ambient temperature is −20 ° C. to 40 ° C.
NO含有排ガスの冷却および酸化は、ガスの滞留時間が約1分以上であるように定寸されたエージング反応器(aging reactor)中で行われ得る。 Cooling and oxidation of the NO-containing exhaust gas can be performed in an aging reactor sized so that the residence time of the gas is about 1 minute or more.
一実施形態において、酸化反応は、NOのNO2への酸化を促進する触媒の存在下で行われる。これらの触媒は当技術分野で公知であり、TiO2上のPt、SiO2上のPt、ならびにアルミナ上の活性炭またはPtおよび/もしくはPdを含む。 In one embodiment, the oxidation reaction is carried out in the presence of a catalyst that promotes the oxidation of NO to NO 2 . These catalysts are known in the art and include Pt on TiO 2 , Pt on SiO 2 , and activated carbon or Pt and / or Pd on alumina.
上述のように、所望されるFast SCR反応には等量のNOとNO2が必要とされる。したがって、250℃未満の温度で煙道ガスに注入されるNO2の量は、SCR触媒ユニットの入口で、煙道ガス中の窒素酸化物含有量の45~55体積%がNO2になるように制御される。 As mentioned above, the desired Fast SCR reaction requires equal amounts of NO and NO 2 . Therefore, the amount of NO 2 injected into the flue gas at a temperature below 250 ° C. is such that 45 to 55% by volume of the nitrogen oxide content in the flue gas is NO 2 at the inlet of the SCR catalyst unit. Is controlled by.
別の態様において、本発明は、本発明による方法における使用のためのシステムを提供する。 In another aspect, the invention provides a system for use in the method according to the invention.
システムは、煙道ガスダクト内に、窒素酸化物の選択的還元用触媒で触媒された1つもしくは複数のファブリックフィルターバッグを有するフィルターバッグハウス;
1つもしくは複数のファブリックフィルターバッグまたはフィルターバッグハウスの上流に、アンモニアまたは尿素溶液の煙道ガスダクトへの注入のための注入手段;
1つもしくは複数のファブリックフィルターバッグまたはフィルターバッグハウスの上流に、二酸化窒素含有排ガスの注入のための注入手段;ならびに
煙道ガスダクトの外側に、
アンモニア酸化触媒ユニット、および
その出口端で二酸化窒素含有排ガスの注入のための注入手段に接続された、アンモニア酸化触媒から回収された一酸化窒素含有排ガスを冷却および酸化して二酸化窒素含有排ガスにするための手段
を含む。
The system is a filter bag house with one or more fabric filter bags catalyzed by a catalyst for selective reduction of nitrogen oxides in a flue gas duct;
A means of injecting ammonia or urea solution into a flue gas duct upstream of one or more fabric filter bags or filter bag houses;
Injection means for injecting nitrogen dioxide-containing exhaust gas upstream of one or more fabric filter bags or filter bag houses; as well as outside the flue gas duct.
The nitric oxide-containing exhaust gas recovered from the ammonia oxidation catalyst, which is connected to the ammonia oxidation catalyst unit and the injection means for injecting the nitrogen dioxide-containing exhaust gas at its outlet end, is cooled and oxidized to the nitrogen dioxide-containing exhaust gas. Including means for.
上述のように、NOのNO2への酸化反応には、少なくとも1分間のNO含有ガスの滞留時間が必要とされる。典型的には1~2分である。 As described above, the oxidation reaction of NO to NO 2 requires a residence time of NO-containing gas for at least 1 minute. Typically 1-2 minutes.
これは、ガス冷式または水冷式のいずれかの熱交換器において、または成形する場合、所望の滞留時間でガスが管を通るような長さを有する渦巻き管のような冷却および酸化手段において実現され得る。 This is achieved in either gas-cooled or water-cooled heat exchangers, or in cooling and oxidizing means such as swirl tubes that, when molded, have a length that allows the gas to pass through the tube with the desired residence time. Can be done.
別の実施形態において、一酸化窒素含有排ガスを冷却および酸化する手段は、NOのNO2への酸化を促進する酸化触媒を備えている。 In another embodiment, the means for cooling and oxidizing the nitric oxide-containing exhaust gas comprises an oxidation catalyst that promotes the oxidation of NO to NO 2 .
Claims (9)
煙道ガスに添加されたアンモニアそれ自体またはその前駆体の形態のいずれかの存在下で、煙道ガスを窒素酸化物の選択的還元用触媒を有する1つもしくは複数のファブリックフィルターバッグに通すステップ;
1つもしくは複数のファブリックフィルターバッグの上流で、二酸化窒素を含有する排ガスを煙道ガスに注入するステップ;
酸化触媒の存在下で、アンモニアまたはその前駆体を酸素含有雰囲気下で触媒酸化して、一酸化窒素および酸素を含有する排ガスにするステップ、
一酸化窒素および酸素を含有する排ガスを周囲温度まで冷却し、冷却された排ガス中の一酸化窒素を酸化して、二酸化窒素を含有する排ガスにするステップ
により、二酸化窒素を含有する排ガスを得るステップ
を含む、方法。 A method of removing nitrogen oxides from the flue gas of combustion equipment.
The step of passing the flue gas through one or more fabric filter bags with a catalyst for the selective reduction of nitrogen oxides in the presence of either ammonia itself added to the flue gas or in the form of its precursors. ;
Injecting nitrogen dioxide-containing exhaust gas into flue gas upstream of one or more fabric filter bags;
A step of catalytically oxidizing ammonia or its precursor in the presence of an oxidation catalyst in an oxygen-containing atmosphere to produce an exhaust gas containing nitric oxide and oxygen.
A step of obtaining an exhaust gas containing nitrogen dioxide by cooling the exhaust gas containing nitric oxide and oxygen to an ambient temperature and oxidizing the nitrogen monoxide in the cooled exhaust gas to the exhaust gas containing nitrogen dioxide. Including the method.
The method according to claim 1, wherein the oxygen -containing atmosphere is ambient air.
煙道ガスダクト内に、窒素酸化物の選択的還元用触媒を有する1つもしくは複数のファブリックフィルターバッグを有するフィルターバッグハウス;
1つもしくは複数のファブリックフィルターバッグまたはフィルターバッグハウスの上流に、アンモニアまたは尿素溶液の煙道ガスダクトへの注入のための注入手段;
1つもしくは複数のファブリックフィルターバッグまたはフィルターバッグハウスの上流に、二酸化窒素含有排ガスの注入のための注入手段;ならびに
煙道ガスダクトの外側に、
アンモニア酸化触媒ユニット、および
その出口端で二酸化窒素含有排ガスの注入のための注入手段に接続された、アンモニア酸化触媒ユニットから回収された一酸化窒素含有排ガスを冷却および酸化して二酸化窒素含有排ガスにするための手段
を含む、システム。 A system for use in the method according to any one of claims 1 to 5.
A filter bag house with one or more fabric filter bags with a catalyst for the selective reduction of nitrogen oxides in the flue gas duct;
A means of injecting ammonia or urea solution into a flue gas duct upstream of one or more fabric filter bags or filter bag houses;
Injection means for injecting nitrogen dioxide-containing exhaust gas upstream of one or more fabric filter bags or filter bag houses; as well as outside the flue gas duct.
The nitric oxide-containing exhaust gas recovered from the ammonia oxidation catalyst unit , which is connected to the ammonia oxidation catalyst unit and the injection means for injecting the nitrogen dioxide-containing exhaust gas at its outlet end, is cooled and oxidized into the nitrogen dioxide-containing exhaust gas. A system that includes means to do.
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